Carbon flux models that are largely driven by remotely sensed data can be used to estimate gross primary productivity (GPP) over large areas, but despite the importance of peatland ecosystems in the global carbon cycle, relatively little attention has been given to determining their success in these ecosystems. This paper is the first to explore the potential of chlorophyll-based vegetation index models for estimating peatland GPP from satellite data. Using several years of carbon flux data from contrasting peatlands, we explored the relationships between the MERIS terrestrial chlorophyll index (MTCI) and GPP, and determined whether the inclusion of environmental variables such as PAR and temperature, thought to be important determinants of peatland carbon flux, improved upon direct relationships. To place our results in context, we compared the newly developed GPP models with the MODIS (Moderate Resolution Imaging Spectrometer) GPP product. Our results show that simple MTCI-based models can be used for estimates of interannual and intra-annual variability in peatland GPP. The MTCI is a good indicator of GPP and compares favorably with more complex products derived from the MODIS sensor on a site-specific basis. The incorporation of MTCI into a light use efficiency type model, by means of partitioning the fraction of photosynthetic material within a plant canopy, shows most promise for peatland GPP estimation, outperforming all other models. Our results demonstrate that satellite data specifically related to vegetation chlorophyll content may ultimately facilitate improved quantification of peatland carbon flux dynamics.